Modeling studies on photochemical combustion reversal: using H2O to hydrogenate CO2

任何燃料或任何有机材料的燃烧都会从大气中吸收氧气并产生CO2和H2O。可以通过使用光化学输入来恢复该过程。换句话说，CO2和H2O的照射以及在合适的催化剂存在下能够释放氧气并重整有机材料，其进而可以用作标准发动机或燃料电池的燃料。执行这种显着的转换的可能性仅限于微尺度和极少数的选择性系统。最近的文献声称，至少可以将选择性提高到理想水平。不幸的是，迄今为止，这些非凡过程的活动和规模都没有超过实验室规模。我们提出了一个机制/建模研究，旨在了解现有的系统之一。特别是，我们选择了基于BiVO 4的光系统，因为它不需要任何电化学输入来生产乙醇。该项目分为三个分项目，分别旨在： 1.分析和改进现有的催化系统，以引入用于催化剂性能改进的修改; 2：对催化剂活性位点进行建模研究，以了解CO2还原如何沿着O2的演变。这项工作有望产生数据，这些数据可能是未来催化剂设计和改进的进一步灵感的基础; 3.分析了CO2催化生成C-C键的因素。这将通过制备与光电导BiVO 4相关的分子系统来进行。再一次的理解，预计将产生宝贵的信息，指导未来的研究，旨在发现更有效的催化系统。

Combustion of any fuel, or of any organic material, uptakes oxygen from the atmosphere and generates CO2 and H2O. It is possible to revert the process by using a photochemical input. In other words, the irradiation of CO2 and H2O and in the presence of an appropriate catalyst is capable of releasing oxygen gas and reforming organic material, which in turn can be used as a fuel for standard engines or fuel cells. The possibility of performing such a remarkable transformation is solely limited to micro-scale and a very few selective systems. Recent literature claims indicated that it is at least possible to improve the selectivity to ideal level. Unfortunately though, the activity and scale of such remarkable processes so far do not exceed the lab scale. We propose a mechanistic/modeling study aiming at understanding one of the existing systems. In particular we have selected the photosystem based on BiVO4 due to the fact that it does not require any electrochemical input for the production of ethanol. The project is organized in three sub-projects aiming respectively at: 1: analyzing and improving the existing catalytic systems to introduce modifications for catalyst performance improvements; 2: modeling studies on the catalyst active site to understand how the CO2 reduction occurs along with the O2 evolutions. This work is expected to produce data that may be the foundation for further inspiration about future catalyst design and modification; 3: analyzing the factors catalytically generating C-C bond from CO2. This will be carried out by preparing molecular systems related to the photosemiconducting BiVO4. Once again understanding is expected to generate precious information for guiding future research aiming at the discovery of more performing catalytic systems.